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Light-wave coherent control of the insulator-to-metal transition in a strongly correlated material

Rui E. F. Silva, Eduardo B. Molinero

Published Jun 2, 2022• 0 citations
Publisher

Abstract

Abstract The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shinning a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering an insulator-to-metal phase transition. In this work, we take advantage of the threshold character of this insulator-to-metal transition and we propose a pump-probe scheme that consists of a mid-infrared laser pulse and a train of short pulses separated by half-period of the mid-infrared with alternating phases. By varying the time-delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, that leaves it fingerprint at its high harmonic spectrum.

DOI
10.21203/rs.3.rs-1687921/v1

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Abstract The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shinning a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering an insulator-to-metal phase transition. In this work, we take advantage of the threshold character of this insulator-to-metal transition and we propose a pump-probe scheme that consists of a mid-infrared laser pulse and a train of short pulses separated by half-period of the mid-infrared with alternating phases. By varying the time-delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, that leaves it fingerprint at its high harmonic spectrum.
The use of intense tailored light fields is the perfect tool to achieve ultrafast control of electronic properties in quantum materials. Among them, Mott insulators are materials in which strong electron-electron interactions drive the material into an insulating phase. When shining a Mott insulator with a strong laser pulse, the electric field may induce the creation of doublon-hole pairs, triggering a photoinduced transition into a metallic state. In this paper, we take advantage of the threshold character of this photoinduced transition and we propose a setup that consists of a midinfrared laser pulse and a train of short pulses separated by a half period of the midinfrared with alternating phases. By varying the time delay between the two pulses and the internal carrier envelope phase of the short pulses, we achieve control of the phase transition, which leaves its fingerprint at its high harmonic spectrum.
Different insulator phases compete with each other in strongly correlated materials with simultaneous local and non-local interactions. It is known that the homogeneous Mott insulator converts into a charge density wave (CDW) phase when the non-local interactions are increased, but there is ongoing debate on whether and in which parameter regimes this transition is of first order, or of second order with an intermediate bond-order wave phase. Here we show that strong-field optics applied to an extended Fermi-Hubbard system can serve as a powerful tool to reveal the nature of the quantum phase transition. Specifically, we show that in the strongly interacting regime characteristic excitations such as excitons, biexcitons, excitonic strings, and charge droplets can be tracked by the non-linear optical response to an ultrafast and intense laser pulse. Subcycle analysis of high harmonic spectra unravels the ultrafast dynamics of these increasingly complex objects, which partially escape the scrutiny of linear optics. Their appearance in the high harmonic spectrum provides striking evidence of a first-order transition into the CDW phase, and makes a strong case for using strong-field optics as a powerful tool to reveal the nature of quasiparticles in strongly correlated matter, and to track the electron dynamics during a first-order quantum phase transition.
The breakdown of a Mott-insulator when subjected to intense laser fields is characterized by the formation of doublon-hole pairs. This breakdown is furthermore evidenced by the production of high harmonics that can be experimentally measured. Here, we present an approach for extracting the doublon-hole correlation length of a Mott insulator. The method is based on a dynamical calculation of the Mott insulator’s rate of charge production in response to an applied strong-field laser pulse. We find that coupling the Mott insulator to a metal drastically increases the correlation length, in support of our recent hypothesis [ Phys. Rev. B 108 , 144434 ( 2023 ) 2469-9950 10.1103/PhysRevB.108.144434 ] that coupling to a metal enhances the charge fluctuations in the insulator. We confirm our conclusions using density matrix renormalization group (DMRG) calculations. The proposed method can be applied to experimentally measured observables, such as differential reflectivity or the high harmonic generation (HHG) spectrum to extract doublon-hole correlation length.
High harmonic generation (HHG) has emerged as a powerful probe of ultrafast electron dynamics in solids. However, in strongly correlated materials, where electronic excitations arise from many-body interactions rather than single-particle band dispersion, the field remains in its infancy. Here, we report HHG up to the 23rd^{rd}rd order in the prototypical Mott insulator La2_22​CuO4_44​. We observe a robust 4 eV cutoff that is independent of driving field strength, revealing an intrinsic energy scale defined by the Hubbard bands. Using time-resolved high harmonic spectroscopy, we disentangle the distinct contributions of carrier creation, intraband acceleration, and interband recombination to the nonequilibrium radiation spectrum. We demonstrate that photo-doping triggers a fundamental reorganization of the many-body manifolds above a critical excitation density, a process that renormalizes the band curvature and suppresses nonlinear intraband currents, thereby directly imprinting the signature of many-body band reconstruction onto the harmonic emission. These results establish HHG as a sensitive probe of subtle correlation-driven electronic reconstructions and highlight that many-body interactions enable extreme nonlinear optical responses that are highly tunable in nonequilibrium states.
Abstract With a combination of numerical methods, including quantum Monte Carlo, exact diagonalization, and a simplified dynamical mean-field model, we consider the attosecond charge dynamics of electrons induced by strong-field laser pulses in two-dimensional Mott insulators. The necessity to go beyond single-particle approaches in these strongly correlated systems has made the simulation of two-dimensional extended materials challenging, and we contrast their resulting high-harmonic emission with more widely studied one-dimensional analogues. As well as considering the photo-induced breakdown of the Mott insulating state and magnetic order, we also resolve the time and ultra-high-frequency domains of emission, which are used to characterize both the photo-transition, and the sub-cycle structure of the electron dynamics. This extends simulation capabilities and understanding of the photo-melting of these Mott insulators in two dimensions, at the frontier of attosecond non-equilibrium science of correlated materials.
We theoretically investigate the dynamics of insulator-metal transition induced by light-pulse excitation in one-dimensional Mott insulators. We adopt the Pariser--Parr--Pople model and the pump-probe signal is obtained by numerically calculating the time development of the state excited by light pulse. When the photoexcitation density is below about 10%, an extremely small portion of the energy eigenstates dominates the optical process and the spin-charge separation holds in these dominant energy eigenstates. As a result, the Mott gap and the short-range antiferromagnetic (AF) spin order are preserved and spin relaxation does not occur. When the density is above the value, a metallic state without the Mott gap is photogenerated and the magnitude of the short-range AF spin order is significantly reduced by photoexcitation. This is consistent with the experimentally observed photoinduced Mott transition. Furthermore, spin relaxation occurs in the metallic state. This photoinduced Mott transition is a manifestation of the spin-charge coupling in the intensely photoexcited states.